| Zn(Ⅱ)金属有机骨架作为基质金属蛋白酶模拟物催化水解微囊藻毒素-LR | |
| A Zn(Ⅱ) metal-organic framework as a matrix metalloproteinase mimic to catalyze the hydrolysis of microcystin-LR | |
| 摘要: 以3-氨基-1，2，4-三氮唑-5-羧酸（Hatz）和1，3，5-苯三甲酸（H3btc）为配体，制备了模拟基质金属蛋白酶（MMPs）结构的纳米片状Zn（Ⅱ）金属有机骨架Zn-MOF-1-NS。Zn-MOF-1-NS能成功实现对微囊藻毒素（MC-LR）肽键的水解。在常温条件下，7.5 h内Zn-MOF-1-NS催化水解了82.6%的MC-LR（k=0.23 h-1），远高于目前报道的具有最高水解效率的菱铁矿（k=0.04 h-1）。研究发现，在该体系中即使添加10倍剂量的腐殖酸，也不会显著阻碍MC-LR的水解，证明Zn-MOF-1-NS对MC-LR的水解具有显著的选择性。通过原位衰减全反射傅里叶变换红外光谱（in-situ ATR-FTIR）、X射线光电子能谱（XPS）分析、理论计算以及与非羧基对应物的比较，发现Zn-MOF-1-NS表面Zn（Ⅱ）位点和羧基共同参与了MC-LR肽键的水解。 | |
| 关键词: 微囊藻毒素-LR 选择性水解 模拟酶 金属有机骨架 基质金属蛋白酶 | |
| 基金项目: 国家自然科学基金（No.22076098，22136003，22376118，21577078）、湖北省自然科学基金杰出青年项目（No.2023AFA054）和地方高校能源和环境材料化学学科创新引智基地（No.D20015）资助 | |
| Abstract: Constructed by the ligands of 3-amino-1,2,4-triazole-5-carboxylic acid (Hatz) and 1,3,5-benzenetricarboxylic acid (H3btc), a Zn(Ⅱ) metal-organic framework with nanosheet morphology (Zn-MOF-1-NS) was prepared to mimic the structures of matrix metalloproteinases (MMPs). Zn-MOF-1-NS was highly effective in catalyzing the hydrolysis of the peptide bonds of microcystin (MC-LR). Within just 7.5 h, 82.6% of MC-LR was hydrolyzed (k=0.23 h-1), which was much higher than the reported best hydrolysis efficiency of siderite (k=0.04 h-1). This research has found that even when the amount of humic acid was increased tenfold, it did not significantly impede MC-LR decomposition. This demonstrates the impressive ability of the catalyst to resist interference from natural organic matter (NOM). Through in-situ attenuated total reflectance Fourier transform infrared spectroscopy (in-situ ATR-FTIR) and X-ray photoelectron spectroscopy (XPS) analyses, theoretical calculations, and comparison with a non-carboxyl counterpart, it was discovered that the surficial Zn(Ⅱ) site and the carboxyl group of Zn-MOF-1-NS participate in the cleavage of the peptide bond. | |
| Keywords: microcystin-LR selective hydrolysis enzyme mimicking metal-organic framework matrix metalloproteinase | |
| 投稿时间：2023-06-30 修订日期：2023-11-02 | |
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| 方艳芬,贺玉婷,赵丽,牛慧斌,陈春城,李悦,黄应平.Zn(Ⅱ)金属有机骨架作为基质金属蛋白酶模拟物催化水解微囊藻毒素-LR[J].无机化学学报,2023,39(12):2265-2278. | |
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| Support information: 相关附件： 20230251_20230251-Supplementary_Information-1031 (1).doc | |
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